Generalizing the Chiral Self-Assembly of Spheres and Tetrahedra to Non-Spherical and Polydisperse Molecules in (C70)x(C60)1–x(SnI4)2

We describe the spontaneous chiral self-assembly of C70 with SnI4 as well as a mixture of C60 and C70 with SnI4. Macroscopic single crystals with the formula (C70)x(C60)1–x(SnI4)2 (x = 0–1) are reported. C60, which is spherical, and C70, which is ellipsoidal, form a solid solution in these crystals, and the cubic lattice parameter of the chiral phase linearly increases as x grows from 0 to 1 in accordance with Vegard’s law. Our results demonstrate that nonspherical particles and polydispersity are not an impediment to the growth of chiral crystals from high-symmetry achiral precursors, providing a route to assemble achiral particles including colloidal nanocrystals and engineered nanostructures into chiral materials without the need to use external templates or forces.